An exploration into potassium (K) containing MoS2 active phases and its transformation process over MoS2 based materials for producing methanethiol

Lu, Jichang; Luo, Yongming; He, Dedong; Xu, Zhipeng; He, Shan; Xie, Delong; Mei, Yi

doi:10.1016/j.cattod.2019.01.012

Cited by 35 publications

(27 citation statements)

References 62 publications

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“…Such intercalation is well known for bulk MoS 2 and results in the interlayer gap expansion according to XRD . This increase was detected for a spent catalyst . using XRD.…”

Section: Discussionmentioning

confidence: 59%

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Effect of Promoter Nature on Synthesis Gas Conversion to Alcohols over (K)MeMoS₂/Al₂O₃ Catalysts

et al. 2020

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The influence of the promoter nature and of a modifier in (K)(Me)MoS2/Al2O3 (Me=Fe, Co, Ni) catalysts on the conversion and selectivity of products of synthesis gas conversion to alcohols and jnl oxygenates was investigated. Relationships between promoter nature, hydrocarbon chain length and selectivity in the formed alcohols were established. Electronic structure of a promoter atom in an active site (AS) was found to strongly affect selectivity of alcohol formation. Promotion of the S‐edge by Fe, Co or Ni suppressed hydrogen activation, which resulted in a lower synthesis gas conversion. Promotion of the M‐edge by Fe, Co, or Ni entailed the formation of double vacancies which are active sites of synthesis gas conversion. Potassium affected the oxophilicity of Mo atoms and reduced Co/Ni‐promoted MoS AS. It decreased the probability of C−O bond breaking in the adsorbed intermediate and shifted selectivity from the formation of alkyl towards alkoxide fragments over these catalysts.

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“…Such intercalation is well known for bulk MoS 2 and results in the interlayer gap expansion according to XRD . This increase was detected for a spent catalyst . using XRD.…”

Section: Discussionmentioning

confidence: 59%

“…[44] This increase was detected for a spent catalyst. [45] using XRD. However, TEM data do not show this increase in anjnl study.…”

Section: Discussionmentioning

confidence: 99%

Effect of Promoter Nature on Synthesis Gas Conversion to Alcohols over (K)MeMoS₂/Al₂O₃ Catalysts

et al. 2020

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“…As the promoter (either Ni or Co) increases electron density of basic S anions, they could favor C-S bonds cleavage. The possibility of electron-rich alumina-lanthana supports contributing to increased sulfur anion basicity (then enhancing the DDS reaction pathway), as recently reported in the case of K-doped MoS 2 phases applied in methanethiol synthesis from a H 2 S-CH 4 mixture [6], remains a question that deserves to be answered. Mechanistic studies on DBT HDS over La-modified alumina supports are clearly needed, as information on reaction routes and kinetic parameters could provide valuable parameters that could be useful in investigations focused on applying that kind of catalyst under more realistic conditions in the presence of oil-derived middle distillates [71].…”

Section: Hds Reaction Testmentioning

confidence: 90%

“…However, decreased activity for organo-S species desulfurization (thiophene) was also observed [4], although in a lower degree, as to that registered for alkenes hydrogenation. Formation of K-decorated and K-intercalated MoS 2 phases supported on SBA-15 mesoporous materials of enhanced activity and selectivity to methanethiol from a H 2 S-CH 4 mixture have been recently reported [6]. According to the authors, electron donation from K atoms could enhance the electron density of sulfided Mo species that facilitated formation of increased amounts of Mo-coordinatively unsaturated sites (CUS).…”

Section: Introductionmentioning

confidence: 99%

Dibenzothiophene Hydrodesulfurization over P-CoMo on Sol-Gel Alumina Modified by La Addition. Effect of Rare-Earth Content

et al. 2019

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Alumina-lanthana (La at 1, 3, or 5 wt%) supports were prepared by sol-gel from Al alkoxide sol where La(NO3)3 was added. Annealed (550 °C) xerogels were characterized by N2 physisorption, thermal analysis (TG-DTA), X-ray diffraction (XRD), scanning electron microscopy- energy dispersive spectroscopy (SEM-EDS), CO2-adsorption studied in IR region, Raman and ultraviolet-vis (UV-vis) spectroscopies. The texture of amorphous binary matrices of high La dispersion was adequate to applications in catalysts for middle distillates hydrodesulfurization (HDS). Generally, the amount and strength of surface basic sites increased with La content in solids. Mo (at 2.8 at. nm−2) and Co (at Co/(Co+Mo) = 0.3) were deposited over carriers by one-pot simultaneous impregnation in the presence of PO43− (P2O5/(NiO+MoO3) = 0.2 mass ratio). Calcined (400 °C) Co-Mo-P impregnated precursors had decreased basicity as to that of corresponding carriers, suggesting strong La-deposited species interaction. As La content in carriers increased Mo=O Raman stretching vibrations shifted to lower wave-numbers (949 to 935 cm−1) suggesting octahedral molybdates coordination change to tetrahedral. Although La at the lowest concentration (1 wt%) enhanced dibenzothiophene, HDS (~38% higher as to the Al2O3-supported formulation) desulfurization was significantly diminished at augmented content. Presence of hardly sulfidable tetrahedral Mo originated during impregnation at basic conditions in pores of La-modified carriers seemed to dictate observed behavior. Rare earth content in formulations enhanced selectivity to biphenyl.

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“…More and more researchers are mainly focused on finding a more economical and environmentally friendly synthesis routes in recent years. Among them, the catalytic synthesis of CH 3 SH from sulfur-containing synthesis gas has aroused great interest among researchers [7][8][9][10][11][12][13][14], but the conversion and yield of CH 3 SH are relatively low, which does not meet the requirements of large-scale industrialization. CS 2 is relatively surplus and the price is low at present, and the one-step synthesis of CH 3 SH by CS 2 hydrogenation has the advantages of low reaction temperature (260~280 • C) and fewer three wastes.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of Methyl Mercaptan on Mesoporous Alumina Prepared with Hydroxysafflor Yellow A as Template: The Synergistic Effect of Potassium and Molybdenum

Peng

Zeng

et al. 2021

Catalysts

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K-promoted Mo-based catalysts showed great promise for the hydrogenation of CS2 to methyl mercaptan (CH3SH). However, the research on the synergistic effect of K and Mo, and the active site of CS2 hydrogenation to CH3SH were unexplored widely. To solve this problem, the synergistic effect of K and Mo in the K-promoted Mo-based catalysts for CS2 hydrogenation to prepare CH3SH was investigated. The mesoporous alumina was the support and loaded the active components potassium and molybdenum to prepare the catalyst. The results suggested that the active components K and Mo can not only cooperatively regulate the acid-base sites on the catalyst surface, but also stabilize the molybdate species at +5 valence during the reduction process and increase the Mo unsaturated coordination sites. Combined with the results of the catalytic activity evaluation, indicating that the main active site of the catalysts is the weak Lewis acid-base site, and the strong acidic site and strong alkaline site are not conducive to the formation of CH3SH. Moreover, the possible catalytic mechanism of CS2 hydrogenation to CH3SH on the weak Lewis acid-base sites of the catalysts was proposed. The research results of this paper can provide an experimental basis and theoretical guidance for the design of high-performance CH3SH synthesis catalyst and further mechanism research.

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An exploration into potassium (K) containing MoS2 active phases and its transformation process over MoS2 based materials for producing methanethiol

Cited by 35 publications

References 62 publications

Effect of Promoter Nature on Synthesis Gas Conversion to Alcohols over (K)MeMoS₂/Al₂O₃ Catalysts

Effect of Promoter Nature on Synthesis Gas Conversion to Alcohols over (K)MeMoS₂/Al₂O₃ Catalysts

Dibenzothiophene Hydrodesulfurization over P-CoMo on Sol-Gel Alumina Modified by La Addition. Effect of Rare-Earth Content

Synthesis of Methyl Mercaptan on Mesoporous Alumina Prepared with Hydroxysafflor Yellow A as Template: The Synergistic Effect of Potassium and Molybdenum

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An exploration into potassium (K) containing MoS2 active phases and its transformation process over MoS2 based materials for producing methanethiol

Cited by 35 publications

References 62 publications

Effect of Promoter Nature on Synthesis Gas Conversion to Alcohols over (K)MeMoS2/Al2O3 Catalysts

Effect of Promoter Nature on Synthesis Gas Conversion to Alcohols over (K)MeMoS2/Al2O3 Catalysts

Dibenzothiophene Hydrodesulfurization over P-CoMo on Sol-Gel Alumina Modified by La Addition. Effect of Rare-Earth Content

Synthesis of Methyl Mercaptan on Mesoporous Alumina Prepared with Hydroxysafflor Yellow A as Template: The Synergistic Effect of Potassium and Molybdenum

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Effect of Promoter Nature on Synthesis Gas Conversion to Alcohols over (K)MeMoS₂/Al₂O₃ Catalysts

Effect of Promoter Nature on Synthesis Gas Conversion to Alcohols over (K)MeMoS₂/Al₂O₃ Catalysts